One of the first examples of a one-pot synthesis of multiblock copolymers via
iterative monomer addition was reported by Whittaker and his co-workers in 201180, 124, 125. Utilising Cu(0)-mediated living radical polymerisation they managed to synthesise high-
Athina Anastasaki 29 order multiblock copolymers comprising very short blocks. Although remarkable, this work reached its limitations when a decablock copolymer was targeted, whereby molecular weight distributions were found to gradually increase (Ð ~ 1.7 for the final decablock copolymer), indicating significant termination events125. Moreover, higher molecular weight polymers were not reported. The same technique was subsequently employed for the synthesis of a number of multiblock glycopolymers which retained very narrow dispersity values101, although quantitative conversion was not achieved in all cases98.
More recently, and in parallel with our own experiments, Perrier and co- workers reported the synthesis of an icasoblock multiblock copolymer consisting of acrylamides both in aqueous and organic media185-188. However, the high temperature (~70 ˚C) that was utilised potentially limits the possibility of simultaneous biological applications while at the same time narrows the monomer pool to only acrylamides, as polymerisation of other monomers (e.g. acrylates) at these temperatures would result in unavoidable termination and side reactions189, 190. Moreover, the addition of external free radical initiator for each monomer addition potentially compromises the integrity of the multiblock copolymers, as it can lead to a small percentage of homopolymer.
Perhaps more importantly, multiblock copolymers, apart from forming functional domains, can also serve as a useful tool to explore and expand the potential as well as to identify the limitations of a given polymerisation system. Careful optimisation of the experimental conditions can provide useful guidelines for performing polymerisations with very high end-group fidelity, even at full monomer conversion, while keeping the dispersity values as low as possible. Of course, we should always remember that in a pseudo-living polymerisation system (such as SET, ATRP or RAFT) which involves radicals, termination will always happen. The challenge is to find the best way to suppress it. As John Maynard Keynes said “In the very long run we are all dead”. Growing polymer
Athina Anastasaki 30 radicals will eventually die. We just do our best to make sure this will happen in a “very, very longrun”, on the timescales of the polymerisation reaction.
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